The solid complexes of some benzylidene aniline containing the p—N(CHS)2 substituent are pre- pared and investigated by ir, electronic absorption and proton magnetic resonance spectroscopy. Molecular compounds with the non-acidic or weak acidic acceptors are fonned through TC- 7Ü,* transition while those with strong acidic acceptors are fcrmed through proton and electron transfer. The reaction with p-nitrophenol occurs through TT—TÜ* CT and intermolecular hydro- gen bonding.